Chemically Pre-Lithiated/Sodiated Reduced Graphene Oxide-Antimony Oxide Composites for High-Rate Capability and Long-Term Cycling Stability in Lithium and Sodium-Ion Batteries

Abstract

Utilizing ultrasonication and microwave irradiation processes, we present a straightforward synthetic route to microwave-irradiated reduced graphene oxide (MrGO)-antimony oxides (Sb₂O₃) composites used as anode materials for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs). Furthermore, after a chemical pre-lithiation (PL) and pre-sodiation (PS) process, PL-MrGO/Li_xSb₂O₃ and PS-MrGO/Na_xSb₂O₃ composites incorporating an inorganic solid electrolyte interface (SEI) layer and amorphous Li_xSb₂O₃/Na_xSb₂O₃ were prepared by drying in an ambient environment. Inorganic SEI, including Li(Na)OH already formed at the defect site where irreversible Li/Na-ion trapping occurs, inhibits the initial irreversible reaction and provides ~100% initial coulombic efficiency. In addition, the amorphous Li_xSb₂O₃ and Na_xSb₂O₃ formed before the 1st discharge process promotes improved cycling stability. For LIB, the reversible capacity of PL-MrGO/Li_xSb₂O₃ anode is 877.7 mA h g⁻¹ at 100 mA g⁻¹ after 150^th cycles and 315.3 mA h g⁻¹ after 3000 cycles at 5000 mA g⁻¹. Also, for SIB, PS-MrGO/Na_xSb₂O₃ represents a reversible capacity of 313.1 mA h g⁻¹ at 1200 mA g⁻¹ after 3000 cycles. This rational structural design, which considers the irreversible reactions that occur during cycling, can be extended to developing other high-performance anode materials.